Ultrafast molecular orbital imaging based on attosecond photoelectron diffraction.

Area of Science:

• Quantum dynamics
• Attosecond science
• Molecular physics

Background:

• Understanding molecular structure and dynamics is crucial in chemistry and physics.
• Attosecond extreme ultraviolet (XUV) pulses enable probing ultrafast electronic processes.

Purpose of the Study:

• To investigate the ultrafast ionization dynamics of molecules using attosecond XUV pulses.
• To explore the potential of molecular attosecond photoelectron diffraction (MAPD) for imaging molecular structures and orbitals.

Main Methods:

• Ab initio numerical simulations of molecular ionization dynamics.
• Analysis of photoelectron momentum distributions (PMDs) generated by linearly polarized attosecond XUV pulses.
• Application of the two-center interference model and an inversion algorithm to interpret diffraction patterns.

Main Results:

• Distinct diffraction patterns were observed in the PMDs of H(2)(+), CO(2), and N(2) when aligned perpendicular to the laser polarization.
• The positions of diffraction patterns accurately correlate with internuclear distances.
• Relative heights of diffraction fringes provide information on molecular orbital structures.
• The two-center interference model successfully reproduces the observed diffraction spectra.
• A simple inversion algorithm allowed for the retrieval of the initial molecular orbital.

Conclusions:

• Molecular attosecond photoelectron diffraction is a powerful technique for high-accuracy imaging of molecular structures and orbitals.
• The study demonstrates the feasibility of retrieving molecular orbital information from experimental data.
• This method offers a novel pathway for direct visualization of molecular electronic configurations.